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NASA NTRSDate not supplied

Satellite Tracking of Shallow Cumulus during CAMP2Ex: The Aerosol and Organization Connection

Shallow moist convection is ubiquitous throughout the tropics and represents a key player in boundary layer processes. Shallow clouds come in many forms, from scattered, short-lived cumulus to organized features that include cold pool boundaries and lines reaching O(100 km) scale lasting several hours. In this study, we explore how cloud morphology and environmental aerosol affect shallow cumulus lifecycle properties. Measuring such influences requires a broad, detailed view of these cloud fields as they grow and decay. Geostationary satellites provide a means to follow the clouds with enhanced spatiotemporal sampling from space. We apply a cloud-tracking tool to study lifecycle properties of shallow cumulus sampled during the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) field campaign of 2019. The mission conducted airborne and shipborne operations over the West Pacific Ocean, in tandem with Rapid Scan imagery from the Advanced Himawari Imager (AHI) on the Japan Meteorological Agency’s (JMA) Himawari-8 satellite. We segment shallow cumulus on AHI 0.5-km visible reflectance during the daylit hours of several research flights that exhibited ideal atmospheric conditions for tracking. We collect the resulting cloud tracks by regions containing airborne sampling of the cloud environments and by two specific segmentation techniques: one optimized for small, disorganized cumulus and the other for larger, organized clouds using suitable thresholds for reflectance and blurring. We present an analysis of cloud lifecycle properties using our dual segmentation approach for various sampled environments of CAMP2Ex. A total of 7 research flights (RFs) exhibited ideal conditions for generating cloud-track ensembles under similar thermodynamic and kinematic profiles but with varying aerosol load. We consider lifetime, track-achieved metrics, and ensemble-fitted growth rates to evaluate the aerosol effect. Cloud elongation, a factor in cloud morphology, is also considered for any potential influence in observed shifts in growth rates. The results suggest that aerosol affects cloud lifecycles more significantly for clouds with larger areas and independent of the elongation factor.

Cloud Tracking↗
NASA NTRS1994

Influence of ocean surface conditions on atmospheric vertical thermodynamic structure and deep convection

The authors analyze the influence of Sea Surface Temperature (SST) and surface wind divergence on atmospheric thermodynamic structure and the resulting effects on the occurrence of deep convection using National Meteorological Center radiosonde data and International Satellite Cloud Climatology Program data for July 1983-July 1985. The onset of deep convection requires not only the existence of positive convective available potential energy (CAPE), but also an unstable planetary boundary layer (PBL). A stable PBL is observed to suppress deep convection even when CAPE is positive. Variations of SST have a major effect on CAPE, but surface wind divergence can also affect deep convection by changing the lapse rate in the lower troposphere and humidity in the PBL. Specifically, when SST is greater than or equal to 28 C, CAPE is always positive, and surface wind divergence does not qualitatively change the buoyancy profile above the PBL. Strong surface wind divergence, however, stabilizes the PBL so as to suppress the initiation of deep convection. In warm SST regions, CAPE is greater than 0 regardless of assumptions about condensate loading, although the pseudoadiabatic limit is more consistent with the observed deep convection than the reversible moist-adiabatic limit under these circumstances. When SST is less than 27 C, CAPE is usually negative and inhibits convection, but strong surface wind convergence can destabilize the inversion layer and moisten the PBL enough to make the atmosphere neutrally stable in the mean. As a result, deep convection is generally enhanced either when SST is greater than or equal to 28 C in the absence of strong surface wind divergence or when strong surface wind convergence occurs even if SST is less than 27 C. The anomalous suppression of deep convection in the warm area of the equatorial west Pacific lying between the intertropical convergence zone (ITCZ) and south Pacific convergence zone (SPCZ) is probably caused by dryness in the PBL and an inversion in that area. The seasonal cycles of deep convection and surface wind divergence are in phase with the maximum solar radiation and lead SST for one to three months in the central Pacific. The change of PBL relative humidity plays a critical role in the changeover to convective instability in this case. The seasonal change of deep convection and associated clouds seems not to have important effects on the seasonal change of local SST in the central Pacific.

Fu, Rong↗
NASA NTRS2015

RACORO Continental Boundary Layer Cloud Investigations: 3. Separation of Parameterization Biases in Single-Column Model CAM5 Simulations of Shallow Cumulus

Climatically important low-level clouds are commonly misrepresented in climate models. The FAst-physics System TEstbed and Research (FASTER) Project has constructed case studies from the Atmospheric Radiation Measurement Climate Research Facility's Southern Great Plain site during the RACORO aircraft campaign to facilitate research on model representation of boundary-layer clouds. This paper focuses on using the single-column Community Atmosphere Model version 5 (SCAM5) simulations of a multi-day continental shallow cumulus case to identify specific parameterization causes of low-cloud biases. Consistent model biases among the simulations driven by a set of alternative forcings suggest that uncertainty in the forcing plays only a relatively minor role. In-depth analysis reveals that the model's shallow cumulus convection scheme tends to significantly under-produce clouds during the times when shallow cumuli exist in the observations, while the deep convective and stratiform cloud schemes significantly over-produce low-level clouds throughout the day. The links between model biases and the underlying assumptions of the shallow cumulus scheme are further diagnosed with the aid of large-eddy simulations and aircraft measurements, and by suppressing the triggering of the deep convection scheme. It is found that the weak boundary layer turbulence simulated is directly responsible for the weak cumulus activity and the simulated boundary layer stratiform clouds. Increased vertical and temporal resolutions are shown to lead to stronger boundary layer turbulence and reduction of low-cloud biases.

parameterization↗
NASA NTRS2012

View-Angle Dependent AIRS Cloud Radiances and Fluctuations: Implications of Organized Cloud Structures for Tropical Circulations

Interactions between wave dynamics and moisture generate clouds in a wide range of scales. Organized cloud structures produce statistically asymmetric radiances and perturbations in AIRS and AMSU-B measurements. With high resolution (approx.14 km beamwidth) and high-sensitivity instruments, these wave-modulated cloud structures can be readily detected from calibrated Levell radiance data. In this study we analyzed eight-year (2003 - 2010) statistics of AIRS cloud-induced radiances and found that in tropical convective regions the ascending (13:30 LST) measurements reveal higher view-angle asymmetry in cloud radiance than the descending (1:30 LST). The daytime asymmetry suggests 10% more cloudiness when the instrument views east, implying tilted and banded structures in most of the anvil clouds to which AIRS is sensitive. Such banded cloud structures are likely a manifestation of embedded westward propagating gravity waves in tropical convective systems. More importantly, organized cloud structures carry asymmetric momentum fluxes in addition to energy fluxes, which must be taken into account for modeling wave-wave and wave-mean flow interactions in tropical circulations.

Wu, Dong L.↗
DOE OSTI2022

Connecting the Radiative Influences of Aerosol upon the Mass Flux Profiles of Shallow Cumuli across the Southeast Atlantic Ocean Basin and its Boundaries (Final Report)

The Atlantic Ocean covers approximately 25% of Earth’s surface and the atmosphere above it is home to a complex array of clouds and aerosols that have important influences on regional and global weather and climate. These influences must be accurately depicted in short range, medium range, seasonal, and climate forecast models. Conditions over the tropical Atlantic are particularly complex due to continental scale plumes of dust from the Sahara Desert and smoke from agricultural burning in Africa that drift across the Atlantic Ocean basin toward the Americas. These plumes are often found meandering in the lower atmosphere above shallow tropical clouds that form above the ocean surface, presumably mingling with these clouds on occasion due to convective mixing processes. Elevated dust and smoke particles absorb incoming sunlight and substantially warm the marine atmosphere in the layer in which they are present. This warming may alter the thermal stability of the marine atmosphere and may throttle or enhance the development of clouds, change their internal structure and the rate at which they precipitate. Alternatively, it may isolate the lower atmosphere from drier layers above enabling water vapor to accumulate near the ocean surface potentially leading to the development of deeper convection. Our study was organized around the principal concept of determining the impact of African smoke and dust plumes upon cloud development at ASI and understanding how a popular shallow convection parameterization used in models responds to the presence of this aerosol. We analyzed observations collected during the US Department of Energy (DOE) Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign using the Atmospheric Radiation Measurement Program’s Mobile Facility #1 (AMF-1), which was deployed to Ascension Island (ASI) in Southeastern Atlantic for a one-year period. Ascension Island is immediately downwind from an African source of these plumes, but far enough removed to enable the lower atmosphere to have reacted to their presence. A main goal of our study was to compute radiative heating rate profiles over Ascension Island and along the trajectory from the biomass burning regions along coastal Africa to Ascension Island. To compute the radiative heating rate due to aerosols and clouds, we employed observed profiles of temperature, humidity, and clouds from LASIC alongside aerosol optical properties from the Modern-era Retrospective analysis for Research and Applications Version 2 (MERRA-2), as input for the Rapid Radiation Transfer Model (RRTM). Radiative heating was also assessed across the southeast Atlantic Ocean using an ensemble of back trajectories from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. We were successful in this effort and the resulting publication is already being cited despite its relatively short lifetime in the literature. The second part of our study involved the process-level representation of the clouds observed over the Southeastern Atlantic in models. Our initial task, upon which the balance of this portion of the study depended, was to evaluate the representativeness of the clouds observed by AMF-1. What orographic influence did Ascension Island have on the measured cloud structure? We set out to answer this question by trying to separate observations that were clearly indicative of orographic forcing from those that were representative of open ocean. The siting of AMF-1, which was 340-m above sea-level on the slope of a steep escarpment, proved demonstrably problematic for cloud process measurements. Despite considerable effort using multiple approaches including artificial intelligence (AI), we were unable to successfully compensate for the orographic forcing present at the AMF-1 site on ASI and, hence, produce process-level summaries of the convective mass flux representative of open ocean over the Southeastern Atlantic. Even though the project has officially ended, we are making a final attempt using two new types of clustering algorithm (i.e., AI) on the recommendation of a former student, who is an expert in this area. Since we have only recently begun to test these new AI schemes, the recommendations from the second part of our project outlined below are based on our experience at the time of this report.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

On the Dependence of Simulated Convection on Domain Size in CRMs

Abstract We present a heuristic model to explain the suppression of deep convection in convection‐resolving models (CRMs) with a small number of grid columns, such as those used in super‐parameterized or multi‐scale modeling framework (MMF) general circulation models (GCM) of the atmosphere. Domains with few grid columns require greater instability to sustain convection because they force a large convective fraction, driving strong compensating subsidence warming. Updraft dilution, which is stronger for reduced horizontal grid spacing, enhances this effect. Thus, suppression of deep convection in CRMs with few grid columns can be reduced by increasing grid spacing. Radiative‐convective equilibrium simulations using standalone CRM simulations with the System for Atmospheric Modeling (SAM) and using GCM‐coupled CRM simulations with the Energy Exascale Earth System Model (E3SM)‐MMF confirm the heuristic model results.

CRM↗
NASA NTRS1985

Simulation of mesoscale convective response

Results are reported from a transfer of thermodynamic and dynamic data downscale from a two-dimensional mesoscale model to a two-dimensional cloud model and a subsequent examination of the differential convective response of the cloud model to a mesoscale structure. The mesoscale model included a high resolution PBL formulation, with convective forces expressed in a profile of exchange coefficients over the height of the PBL and the magnitude of the surface heat flux. Account was also taken of forcing by long- and short-wave radiation, surface forcing by the surface energy budget, the terrain shape, and possible wave reflection at the top boundary. The slab-symmetric cloud model possessed subgrid-scale features, five types of moisture terms, and a subroutine for accretion processes. The mesoscale environment was observed to have a significant impact on convective response, i.e., the vertical velocity and the cloud water. Various factors which were not included in the study and which must be considered are discussed.

Mcnider, R. T.↗
DOE OSTI2022

A Vertically Resolved MSE Framework Highlights the Role of the Boundary Layer in Convective Self-Aggregation

Abstract Convective self-aggregation refers to a phenomenon in which random convection can self-organize into large-scale clusters over an ocean surface with uniform temperature in cloud-resolving models. Previous literature studies convective aggregation primarily by analyzing vertically integrated (VI) moist static energy (MSE) variance. That is the global MSE variance, including both the local MSE variance at a given altitude and the covariance of MSE anomalies between different altitudes. Here we present a vertically resolved (VR) MSE framework that focuses on the local MSE variance to study convective self-aggregation. Using a cloud-resolving simulation, we show that the development of self-aggregation is associated with an increase of local MSE variance, and that the diabatic and adiabatic generation of the MSE variance is mainly dominated by the boundary layer (BL; the lowest 2 km). The results agree with recent numerical simulation results and the available potential energy analyses showing that the BL plays a key role in the development of self-aggregation. Additionally, we find that the lower free troposphere (2–4 km) also generates significant MSE variance in the first 15 days. We further present a detailed comparison between the global and local MSE variance frameworks in their mathematical formulation and diagnostic results, highlighting their differences.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2009

Production of Lightning NO(x) and its Vertical Distribution Calculated from 3-D Cloud-scale Chemical Transport Model Simulations

A 3-D cloud scale chemical transport model that includes a parameterized source of lightning NO(x), based on observed flash rates has been used to simulate six midlatitude and subtropical thunderstorms observed during four field projects. Production per intracloud (P(sub IC) and cloud-to-ground (P(sub CG)) flash is estimated by assuming various values of P(sub IC) and P(sub CG) for each storm and determining which production scenario yields NO(x) mixing ratios that compare most favorably with in-cloud aircraft observations. We obtain a mean P(sub CG) value of 500 moles NO (7 kg N) per flash. The results of this analysis also suggest that on average, P(sub IC) may be nearly equal to P(sub CG), which is contrary to the common assumption that intracloud flashes are significantly less productive of NO than are cloud-to-ground flashes. This study also presents vertical profiles of the mass of lightning NO(x), after convection based on 3-D cloud-scale model simulations. The results suggest that following convection, a large percentage of lightning NO(x), remains in the middle and upper troposphere where it originated, while only a small percentage is found near the surface. The results of this work differ from profiles calculated from 2-D cloud-scale model simulations with a simpler lightning parameterization that were peaked near the surface and in the upper troposphere (referred to as a "C-shaped" profile). The new model results (a backward C-shaped profile) suggest that chemical transport models that assume a C-shaped vertical profile of lightning NO(x) mass may place too much mass neat the surface and too little in the middle troposphere.

Ott, Lesley↗
DOE OSTI2023

Multi-scale Analysis of Surface Heterogeneity Induced Convection on Isentropic Coordinates

This research uses semi-idealized simulations to investigate multi-scale processes induced by the heterogeneity of soil moisture observed during the 2016 Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field campaign. The semi-idealized simulations have realistic land heterogeneity, but large-scale winds are removed. Analysis on isentropic coordinates enables the tracking of circulation that transports energy vertically and facilitates the identification of the primary convective processes induced by realistic land heterogeneity. The isentropes associated with upward motion are found to connect the ground characterized by high latent heat flux to cloud bases directly over the ground with high sensible heat flux, while isentropes associated with downward motion connect precipitation to the ground characterized by high sensible heat fluxes. The mixing of dry, warm parcels ascending from the ground with high sensible heat fluxes and moist parcels from high latent heat regions leads to cloud formation. This new mechanism explains how soil moisture heterogeneity provides the key ingredients such as buoyancy and moisture for shallow cloud formation. We also found that the sub-mesoscale dominates upward energy transport in the boundary layer, while mesoscale circulations contribute to vertical energy transport above the boundary layer. Our novel method better illustrates and elucidates the nature of land atmospheric interactions under irregular and realistic soil moisture patterns.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2020

Impact of Convectively Detrained Ice Crystals on the Tropical Upper Troposphere and Lower Stratosphere

The role of convectively detrained ice crystals on the humidity of the tropical upper troposphere and lower stratosphere (UTLS) is investigated in simulations of cirrus clouds along trajectories launched from the 378K potential temperature level in the tropics. The one-dimensional (vertical) cloud model tracks individual ice crystals through their lifecycle beginning with detrainment from convection, followed by deposition growth, sedimentation and sublimation. Convective influence of the parcels is diagnosed by tracing the trajectories through time-dependent fields of convective cloud-top height adjusted to match the CloudSAT and CALIPSO statistics. Model simulations of UTLS water vapor and cloud fields are evaluated and constrained by comparison with Aura MLS and CALIPSO measurements. Preliminary results indicate sensitivity of the detrained ice crystal lifecycle to atmospheric conditions downstream of convection. Specifically, cooling (high relative humidity and supersaturation) downstream of convection leads to deposition growth and sedimentation of detrained ice crystals, resulting in net dehydration of the UTLS. In contrast, warming (low relative humidity and subsaturation) downstream of convection leads to sublimation of detrained ice crystals and subsequent hydration. As such, the impact of detrained ice crystals on the humidity of the UTLS exhibits distinct spatial variability. Detrained ice crystals predominantly dehydrate the UTLS in the tropical mean. Sensitivities to the convectively detrained ice crystal size and concentration are also examined using measurements from the StatoClim aircraft campaign. The importance of convectively detrained ice crystals will be discussed within the context of the overall contribution of convection to the lower stratospheric humidity.

Ueyama, Rei↗
NASA NTRS1983

The life cycle of a tornadic cloud as seen from a geosynchronous satellite

The life span of a severe storm is on the order of a few hours. Rapid-scan infrared and visible observations from geosynchronous satellites can be useful for studying the life cycle of a severe convective storm. By using artificial colors for pixels representing blackbody temperatures of the cloud top, convective storms can be observed throughout their life cycles. In this paper clouds associated with a tornadic storm, the Ringwood, OK tornado on May 29, 1977, are compared with those without a tornadic storm to illustrate how the infrared and visible observations from a geosynchronous satellite can be used to study the differences in their life cycles. The instability of the air mass and the meteorological background are discussed based on balloon observations.

Hung, R. J.↗
DOE OSTI2023

Evaluating Mesoscale Convective Systems Over the US in Conventional and Multiscale Modeling Framework Configurations of E3SMv1

Organized mesoscale convective systems (MCSs) contribute a significant amount of precipitation in the Central and Eastern US during spring and summer, which impacts the availability of freshwater and flooding events. However, current global Earth system models cannot capture MCSs well and misrepresent the statistics of precipitation in the region. In this study, we investigate the representation of MCSs in three configurations of the Energy Exascale Earth System Model (E3SMv1) by tracking individual storms based on outgoing longwave radiation using a new application of TempestExtremes. Our results indicate that conventional parameterizations of convection, implemented in both low (LR; ~150 km) and high (HR; ~25 km) resolution configurations, fail to capture almost all MCS-like events, in-part because they underestimate high-level cloud ice associated with deep convection. On the other hand, the multiscale modeling framework (MMF; cloud-resolving models embedded in each grid-column of ~150 km resolution E3SMv1) configuration represents MCSs and their annual cycle better. Nevertheless, relative to observations, the E3SMv1-MMF spatial distribution of MCSs and associated precipitation is shifted eastward, and the diurnal timing is lagged. A comparison between the large-scale environment in E3SMv1-MMF and ERA5 reanalysis suggests that the biases during the summer in E3SMv1-MMF are associated with biases in low-level humidity and meridional moisture transport within the low-level jet. The fact that conventional parameterizations of convection, even with high-resolution, cannot capture MCSs over the US suggests that methods with explicit representation of kilometer-scale convective organization, such as the MMF, may be necessary for improving the simulation of these convective systems.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1984

Lightning and related phenomena in thunderstorms and squall lines

During the past few years, cooperative research on storm electricity has yielded the following results of both basic and applied interest: (1) the intracloud to cloud-to-ground flashing ratio can be as great as 40:1; (2) as storm cells in a squall line dissipate, longer flashes become predominant; (3) there are two centers of lightning activity maxima that are vertically separated, the lower maximum at about 5 km and the upper at about 12 km. In addition, (4) storms produce lightning in their upper regions at a high rate; (5) lightning appears to be related in time to convective motions; (6) positive cloud-to-ground flashes occur in the severe stage of storms and in the later, well-developed stage of squall line storms; (7) mesoscale convective complexes have been observed to have cloud-to-ground flashing rates of more than 48/min; and (8) the electric field in anvils well away from the main storm core (more than 60 km) can be very high, more than 94 kV/m.

Rust, W. D.↗
NASA NTRS1992

Integration of satellite and surface data using a radiative-convective oceanic boundary-layer model

A mixing-line boundary-layer model is used to retrieve cloud-top height from satellite-derived cloud-top temperatures, using 700-hPa National Meteorological Center (NMC) analyses and the Comprehensive Ocean and Atmosphere Data Set (COADS) surface data as supporting datasets. Results are compared with the fixed-lapse-rate method of retrieving boundary-layer depth from sea surface temperatures (SST) and cloud-top temperatures. A radiative-convective equilibrium boundary-layer model is used to retrieve boundary-layer structure given SST and surface wind, satellite cloud-top temperatures and cloud fraction, and the 700-hPa NMC thermodynamic analyses. Good agreement is found between the COADS data and the model solutions for low-level temperature and moisture. This suggests that equilibrium boundary-layer models may be of use over remote oceans in the retrieval of boundary-layer structure.

Betts, Alan K.↗
NASA NTRS1999

Improving Reanalyses Using TRMM and SSM/I-Derived Precipitation and Total Precipitable Water Observations

Global reanalyses currently contain significant errors in the primary fields of the hydrological cycle such as precipitation, evaporation, moisture, and the related cloud fields, especially in the tropics. The Data Assimilation Office (DAO) at the NASA Goddard Space Flight Center has been exploring the use of rainfall and total precipitable water (TPW) observations from the Tropical Rainfall Measuring Mission (TRMM) Microwave Imager (TMI) and the Special Sensor Microwave/ Imager (SSM/I) instruments to improve these fields in reanalyses. The DAO has developed a "1+1"D procedure to assimilate 6-hr averaged rainfall and TPW into the Goddard Earth Observing System (GEOS) Data Assimilation System (DAS). The algorithm is based on a 6-hr time integration of a column version of the GEOS DAS. The "1+1" designation refers to one spatial dimension plus one temporal dimension. The scheme minimizes the least-square differences between the satellite-retrieved rain rates and those produced by the column model over the 6-hr analysis window. The control variables are analysis increments of moisture within the Incremental Analysis Update (IAU) framework of the GEOS DAS. This 1+1D scheme, in its generalization to four dimensions, is related to the standard 4D variational assimilation but differs in its choice of the control variable. Instead of estimating the initial condition at the beginning of the assimilation cycle, it estimates the constant IAU forcing applied over a 6-hr assimilation cycle. In doing so, it imposes the forecast model as a weak constraint in a manner similar to the variational continuous assimilation techniques. We present results from an experiment in which the observed rain rate and TPW are assumed to be "perfect". They show that assimilating the TMI and SSM/I-derived surface precipitation and TPW observations improves not only the precipitation and moisture fields but also key climate parameters directly linked to convective activities such as clouds, the outgoing longwave radiation, and the large-scale circulation in the tropics. In particular, assimilating these data types reduce the state-dependent systematic errors in the assimilated products. The improved analysis also leads to a better short-range forecast, but the impact is modest compared with improvements in the time-averaged fields. These results suggest that, in the presence of biases and other errors of the forecast model, it is possible to improve the time-averaged "climate content" in the assimilated data without comparable improvements in the short-range forecast skill. Results of this experiment provide a useful benchmark for evaluating error covariance models for optimal use of these data types.

Hou, Arthur Y.↗
DOE OSTI2026

Process‐Oriented Calibration of a Turbulence Scheme in the DOE's Global Storm‐Resolving Model Using Machine Learning

A process‐oriented calibration framework is developed for the Simplified Higher‐Order Closure (SHOC) turbulence scheme in DOE's Simple Cloud Resolving E3SM Atmospheric Model (SCREAM). This framework leverages machine learning surrogates and observational constraints to efficiently calibrate SHOC adjustable parameters across two convective regimes: clear‐sky dry convective boundary layer and fair‐weather shallow cumulus clouds from ARM observations. We use perturbed‐parameter ensembles of a doubly periodic version of SCREAM to train surrogates and apply Markov Chain Monte Carlo sampling guided by cost functions based on benchmarking large‐eddy simulations and observations to identify optimized parameter sets that perform well in both regimes. The calibrated SHOC parameters substantially improve boundary‐layer turbulence and cloud boundaries, and modeled cloud fraction and radiative effects align better with observations than the default. These results demonstrate that combining multiple process‐specific convective regimes with machine‐learning surrogates can reduce parametric uncertainties and yield a model more faithful to cloud–turbulence interactions.

58 GEOSCIENCES↗
DOE OSTI2025

Simulating Droplet-Resolved Haze and Cloud Chemistry Forming Secondary Organic Aerosols in Turbulent Conditions within Laboratory and Cloud Parcels

Most of our existing knowledge of cloud chemistry in regards to forming secondary organic aerosols (SOA) is based on measurements in bulk aqueous solutions. However, SOA reaction kinetics derived from bulk solution measurements might differ from the kinetics in actual cloud droplets, since turbulent mixing and ionic strengths, and ratio of surface area to volume in individual cloud droplets might vary substantially from bulk solutions in the real atmosphere. Three-dimensional models at various scales have been used to simulate aqueous chemistry. However, most of these models do not resolve turbulence down to the smallest length scales of 1 mm and do not simulate cloud chemistry in individual cloud droplets due to large computational costs. Here we incorporate the formation of isoprene epoxydiol SOA (IEPOX-SOA) in individual droplets within a one-dimensional explicit mixing parcel model (EMPM-Chem). We apply EMPM-Chem to simulate turbulence and droplet-resolved IEPOX-SOA formation using a configuration based on the Michigan Tech Pi chamber. We find that the dissolution of IEPOX gases is weighted more towards larger cloud droplets due to their large liquid water content (compared to smaller droplets), while the conversion of dissolved IEPOX to IEPOX-SOA is much greater within smaller deliquesced haze particles due to their higher acidity and ionic strengths compared to cloud droplets. We also find that as droplet residence times increase in the chamber, e.g., due to increasing ammonium bisulfate seed aerosol injection rates and/or increasing heights of the chamber, formation of IEPOX-SOA increases substantially. Thus, our EMPM-Chem model could be used to design future cloud chambers to maximize SOA production from cloud chemistry. We also apply the EMPM-Chem model to simulate how IEPOX-SOA formation evolves in individual cloud droplets within rising cloudy parcels in the atmosphere. We find that as subsaturated air is entrained into and turbulently mixed with the cloud parcel, evaporation causes a reduction in droplet sizes, which leads to corresponding increases in per droplet ionic strength and acidity. Increased droplet acidity in turn greatly accelerates the kinetics of IEPOX-SOA formation. In conclusion, our results provide key insights into single-cloud-droplet chemistry, suggesting that entrainment mixing may be an important process that increases SOA formation in the real atmosphere.

54 ENVIRONMENTAL SCIENCES↗